3.4 ESTUDIO DE DIVERSOS AUTORES
3.4.7 Emilio Jiménez 24
noted that in Heringa et al. (2011) [175] the equivalent ageing time was only 5 h and SOA-EFs are related to flaming phases. Hence, lower primary emissions are also associated with lower SOA SOA factors could be obtained which represent ageing products for each of the considered oxidising agents. Additionally, two factor of POA were obtained, which either contain primary species reacting with all oxidising agents (double bond containing species, BBOA) or only with OH and NO3 radicals (saturated compounds, HOA). During dark ageing, O3 and NO3 oxidise the aerosol, leading to SOA and aged-POA with lower average carbon oxidation state than from ageing with OH radicals [185]
and substantial formation of organonitrates, which were derived from a high ratio of NO+ to NO2+ in the SP-AMS spectrum. ON formation was previously observed in ambient air studies [186, 187], but can now be linked to ageing of wood combustion emissions.
4.4.2 Ageing of primary emissions from pellet combustion in a PAM flow reactor Few experiments with PB emissions in a smog
chamber revealed that no SOA was formed, which was later confirmed in a more comprehensive study by Kari et al. (2017) [188]
and also agrees with previously published SOA yields from a pellet burner [175]. On that account, a PAM flow reactor which is capable to expose the combustion aerosol to higher OH concentration was used, but also led to only insignificant increase in OA mass for the PB operating under optimised conditions (OPT).
Nevertheless, oxygen-to-carbon ratios (O:C) were distinctly enhanced, indicating relevance of heterogeneous oxidation reactions and the formation of aged-POA. However, the equivalent concentration of carbonate carbon to OC and EC contributes to peaks at m/z 44 (CO2+) and m/z 30 (CO+), which may bias the result of OM and explain O:C as well as average carbon oxidation states [4] outside the range of typical values observed in ambient air. To simulate PB of older technology, the secondary
Fig. 25 Van Krevelen diagram of aged (red) and non-aged OA (blue) from optimized combustion conditions (OPT, circles) and reduced secondary air supply (RSA, squares). Solid purple lines belong to slopes indicating main functionalisation of OA [2], where the black lines represent slopes from non-aged to aged OA
Summary and outlook
air supply was reduced by approximately 30% (reduced secondary air, RSA). Hence, organic emissions increased, especially volatile and intermediate-volatile aromatic hydrocarbons, which are considered as potent precursors for SOA formation [189]. In contrast to the PB at full secondary air supply, OA mass was doubled associated with increased relative amounts of the fragment ions C2H3O+ (m/z 43), CO2+ (m/z 44) and C2H4O2+ (m/z 60), which belong to typical SOA compound classes of non-acid oxygenates, carboxylic acids and long-chain carboxylic acids.
The obtained increases of OA mass were converted in to SOA-EFs and compared with the single precursor approach by Bruns et al. (2016) [189]. For OPT, experimental SOA-EFs covered 30% of SOA-EFs obtained from single precursors, while for RSA it was even only 10%. Slopes close to 0.5 in the Van-Krevelen diagram indicate that C-C-bond cleavages occurred during ageing, leading to reaction products of higher volatility than the primarily emitted precursors, which may explain the large discrepancies between the different approaches. Altogether, the overall formation of SOA was low for both OPT and RSA compared to SOA formation from logwood stoves and expected to be negligible with ongoing advances in combustion technology.
5 Summary and outlook
Although the vast majority of aerosol originates from natural sources, combustion aerosols play a key role for climate and air pollution. In particular, emissions from ship traffic and wood combustion gained increasing public attention during the last decade and were investigated within the framework of the DACH-project WOOSHI (“WOOd combustion and SHIpping”). One focus of this study was put on the identification of marker substances by chemometric approaches, which allows the detection and quantification of emission sources by receptor models, such as positive matrix factorisation and chemical mass balance.
In 2015, the fuel sulphur content (FSC) of marine fuels was restricted to 0.1% in coastal areas of Europe and North America (sulphur emission control area), which forces the ship owners to switch from heavy fuel oil (HFO) with an average FSC of 2.7% to marine gas oil (MGO) or diesel fuel (DF).
In particular the composition of the organic emissions from both HFO and MGO/DF is unknown, which was examined by advanced mass spectrometric techniques. In accordance with the high contribution of unburned fuel to the total emissions, mass spectra of particulate organic matter revealed the dominance of homologue series of several compound classes, such as alkylated PAHs, alkylated heterocycles and alkanes. A shift to organic compounds of higher volatility when going from HFO to DF was also observed as well as a general reduction in organic emissions could be observed with DF, but emissions of soot particles measured as elemental carbon (EC) remained stable. Furthermore, evidence was found that ships are a substantial emitter of brown carbon.
Consequences for direct effects on climate by affecting radiative forcing will be discussed in a future publication. Since markers for ship emissions are based on HFO emissions, complementary multivariate statistical analyses were performed with emission profiles of aromatic (intermediate-)volatile organic compounds from ships, road traffic and residential heating in a meta-analysis. Alkylated PAHs were found to discriminate well between land-based and ship emissions
with high statistical significance, independently from the used marine fuel, while the ratio of C2- to C1-naphthalene as an easy-to-use metric allows a first estimation of high ship impact on air pollution.
In an ageing experiment with a mobile smog chamber, no significant increase in organic aerosol mass was detected, thus further investigations involving potential aerosol mass flow reactors are recommended.
Contrary to ships, primary wood combustion emissions are comparably well investigated, but have changed with ongoing advances in combustion technology, such as secondary air supply by air staging or automatically-fired pellet boilers. Appliances with such new combustion technology burn efficiently while reducing organic emissions. Especially the release of primary decomposition products from carbohydrates and lignin is decreased. Hence, simple approaches based on ratios of phenolic species to organic carbon (OC) or OC to EC for identifying the fraction of wood combustion in ambient air are heavily biased, in particular for pellet boilers. Inorganic PM constituents or latent variables from multivariate statistical analyses containing several organic PM constituents may provide more reliable results. Additionally, burning conditions in terms of proper ignition and burning stadia were found to considerably affect the emission profile and results from PMF or CMB.
Besides reduction in primary emissions, the potential of secondary organic aerosol (SOA) formation, investigated with smog chamber and flow reactor, also declines with advances in combustion technology. However, it still exhibits a substantial increase of additional organic aerosol for the modern logwood stove by gas-to-particle conversion and heterogeneous oxidation. Simulation of nighttime atmospheric processing suggests a substantial contribution of logwood combustion SOA to ambient organonitrate concentrations. For the pellet boiler emissions, the SOA formation was negligible even at high exposures of OH radicals although increases in average carbon oxidation state indicated heterogeneous oxidation.
Altogether, this thesis explored the chemical composition of the rarely investigated but relevant emissions by ship, considered advances in wood combustion technology and gave valuable implications for the identification and quantification of wood combustion and ship traffic in source apportionment. The results emphasise the necessary connection between primary and secondary emissions as well as combustion, atmospheric, biological and mathematical science to understand complex effects and consequences from changes of the atmospheric composition on the total environment.
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